Enhanced Chemical Synthesis at Soft Interfaces: A Universal Reaction-Adsorption Mechanism in Microcompartments

被引：231

作者：

Fallah-Araghi, Ali ^{[1
]}

Meguellati, Kamel ^{[1
]}

Baret, Jean-Christophe ^{[2
]}

El Harrak, Abdeslam ^{[3
]}

Mangeat, Thomas ^{[3
]}

Karplus, Martin ^{[1
,4
]}

Ladame, Sylvain ^{[1
,5
]}

Marques, Carlos M. ^{[6
]}

Griffiths, Andrew D. ^{[1
,7
]}

机构：

[1] Univ Strasbourg, ISIS, CNRS UMR 7006, F-67083 Strasbourg, France

[2] Max Planck Inst Dynam & Self Org, D-37077 Gottingen, Germany

[3] Raindance Technol France, F-67083 Strasbourg, France

[4] Harvard Univ, Dept Chem & Chem Biol, Cambridge, MA 02138 USA

[5] Univ London Imperial Coll Sci Technol & Med, Dept Bioengn, London SW7 2AZ, England

[6] Univ Strasbourg, Inst Charles Sadron, CNRS UPR 22, F-67034 Strasbourg, France

[7] Ecole Super Phys & Chim Ind Ville Paris ESPCI Par, CNRS UMR 7084, F-75231 Paris 05, France

来源：

PHYSICAL REVIEW LETTERS | 2014年 / 112卷 / 02期

基金：

欧洲研究理事会;

关键词：

WATER; CONFINEMENT; SURFACTANTS; PARTICLES; CHEMISTRY; EMULSIONS; KINETICS; ORIGIN; LIFE;

D O I：

10.1103/PhysRevLett.112.028301

中图分类号：

O4 [物理学];

学科分类号：

0702 ;

摘要：

A bimolecular synthetic reaction (imine synthesis) was performed compartmentalized in micrometer-diameter emulsion droplets. The apparent equilibrium constant (K-eq) and apparent forward rate constant (k(1)) were both inversely proportional to the droplet radius. The results are explained by a noncatalytic reaction-adsorption model in which reactants adsorb to the droplet interface with relatively low binding energies of a few k(B)T, react and diffuse back to the bulk. Reaction thermodynamics is therefore modified by compartmentalization at the mesoscale-without confinement on the molecular scale-leading to a universal mechanism for improving unfavorable reactions.

引用

页数：5

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